Synthetic production of bodies from



July 17, 1934. R. s. RICHARDSON Re. 19,243`

SYNTHETIC LPRODUCTION OF BODIES FROM THEI-R COMPONENI` GASES I original Filed Apri1,24. 1925 I a Qns our/fr- *u ins fa/M7 7b ciruysf mmm/vg 'Qns ZZ ATTORNEY 'astma .my 11,1934

19.243 -SYNTHETIC PRODUCTION F BODIES THEIR COMPONENT GASES muni; s. Richardson, scandale, N.

Y.. assigner,

by mesnc assignments, to Chemical Engineering Corporation, New Y N. Delaware on' Y., a corporation ofI Orlginal No. 1,704,214, dated March 5, 1929, Berlal No. 25,590, April 24, 1925.

Application for rcllene October 20, 1932, Serial No. 638,8# 1

11 Chime. (Cl. 23-199) My invention relates broadly to processes for converting given substances into others having different physical or chemical characteristics as through the use of a catalytic agent. More par- 5 ticularly my invention comprises novel processes in the manufacture of valuable products by direct synthesis from their component gases which are passed at high temperatures under pressure over a catalyst mass, as for example, the manufacture of methyl alcohol or methanol (CI-LDH) from carbon monoxide (CO) and hydrogen, or the production of synthetic ammonia (NH3) from a gaseous mixture of nitrogen and hydrogen in their combining proportions.- In any instance the elements should be combined in their respective proportions in the gaseous mixture and then compressed to relatively high pressures and passed under such pressure over a suitable catalytic agent capable of stimulating the combination of the two gases whereby sufiicient heat is produced to maintain the temperatures required for satisfactory yields.

In the manufacture of methanol from a mixture of one part of carbon monoxide and two parts of hydrogen by volume which is preferably passed under 300 atmospheres pressure and at a high temperature (300 to 400 C.) over a catalyst containing metallic copper and zinc oxide with recirculation of the uncombined gases, success depends almost entirely on the regulation and control of the temperatures maintained within the catalytic chamber.

In the manufacture of synthetic ammonia industrially by passing the puried gas mixture of nitrogen and hydrogen under the high pressures required through a suitable catalyst, preferably reduced iron oxide heated to a high temperature, say 400 C. to 600 C., with recirculation of the uncombined gases through the apparatus, satisfactory production depends largely, if not almost entirely, upon similar control of the temperatures within the catalyst containers. l

In industrial operations many diiilculties are s encountered in maintaining the catalyst at an optimum temperature after being initially heated from within, since variations of such temperature in either direction lowers the conversion etliciency a of the catalyst with decreased yields. It has'been found that too low temperatures greatly decrease the activity of the catalyst, so that cooling takes place below that required to maintain the reaction, and therefore production of methanol or ammonia ceases entirely. Under ordinary conditions u of operation the heat produced in the catalyst chamber is insuicient to maintain the reaction unless the ingoing gas mixture is preheated either directly or by the hot outgoing mixture after conversion through heat-exchange apparatusk either separately installed or arranged within the catalyst chamber.

Furthermore in industrial practice on a commercial scale, it has been found that the portion-of the catalyst which rst comes in contact with the gas mixture where the activity is more intense, may become injured by overheating or even poisoned by impurities in the gases. Even though such heat is removed by suitable cooling surfaces surrounding that portion oi the catalyst, yet local lover-heating is likely to occur in the catalyst mass. Hence it follows that the maximum life of a catalyst as well as maximum conversion of the synthetic products are largely dependent upon the temperature at.which such catalyst operates in producing methanol orammonia as I have stated.

Heretofore removal of the heat of reaction has been accomplished throughout the catalyst in practice by use of heat transfer surfaces suitably disposed within the catalyst mass, but such system of control inevitably permits great differences in temperature in various isolated parts of the catalyst mass,'and especially allows no adequate control of temperature capable of being varied with operating conditions to secure optimum temperatures for maximum conversion.

According to my invention I control the temperature throughout the catalyst mass in varying sections or zones by which the temperature in the major portion which is last to -be reached by the proper gaseous mixture is'maintained closely to the optimum temperature for maximum methanol or ammonia conversion, since the greater part of the heat generated through the reaction is liberated in the lesser portion of the catalyst mass which initially comes in 'contact with the gas mixture entering the catalyst furnace. The temperature control may be attained by passing comparatively cool gas at various points within the'converter to be circulated therein. Furthermore the temperature in the first section or portion of the catalyst mass is' controlled partly by introducing part of the in-fiow ing gas mixture beyond a portion of the heatexchange surface usually attached to the catalytic furnace and partly by the transfer of heat from the catalyst itself to the incoming flow of the gas mixture, while the temperature of the second, and preferably the major. portion of the w w .w n mmmmmmmmmmwmmmmmm Mmm .m wm m Mmmm@ N Mmmm www mmmmwmmmmw, wmm Wmmfmm www mhmmmm mmhmmmmmmmm i w. mm, @mmmmmmmmmm mmmmmmmmmmmm 1 a m .m .g m ,m @www mmwmmmmmm um m mmmmmmmmmmmmm w am m mmmmmmmmm m W mm mmmmwmmw .mmm mf Mmmm www s mam www mmmmmm m www mmmmmmmmmmmm a www n? mmm .mmh www separate porticnaot onirdesired the m m m m M m m m m m w m m mvmmwmwumwnmwfmlmmmmm fmwmmwwp mwmmwmmmwm m mm mmmmmmmmmmmmmmmmm e.. mmd www3 mmwcmmmwmm wie mmmmmmmmmmmnmmmwmmwdymmmwmmm mmmmmmmnmmmw mem m... mnwnwmmmm bem Emo mmmmmmmmmumwwmm m mmmmm mmmmm mmmqmmmmmwmmw mmmwmmmnmmmm mmwcm., mme mmmwm ,.mmmw www M mmmwwemmmmmmmmmmmmmwm mmmmhmmmmmmmmmm c It. e mp acm ....wt om? u Wmymmmmmmmmmmwmmmmmmmmmmmm mmmnmmmmwmmmmmm ,mb una 6 We ma wm o .mouwumumml vmmmmmmmmmm m mmmmwmmm mman m mmm mn; wmmmecmm pmm w mt e um mm m u wymmmrvmm m25@ fm Wu emam mi mm .u bmrmce e mm mm em w. .www mwmmmmwm @www mmmmmmmmmmmmmmmmmm J .m n e t E r. a I? c mmmmmmmmmmwmm mmmdmmmmmmmmmmwmmnmmmwmmmmmmw .Mmmmm m m euhm r3e. t $8. .ed8M.ew.m8w7..Mn m.v.edhe .d

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l. 'Ihe process of producing ammonia by passing a gaseous mixture of nitrogen and hydrogen over a catalyst mass at high temperatures under pressures below 400 atmospheres which comprises rst passing nitrogen hydrogen mixture through a separated portion of the catalyst mass, then introducing cooler nitrogen hydrogen mixture to the outfiowing mixture and thereafter passing the combined gas ow mixture through another separated portion oi' the catalyst of greater content than saidrst-mentioned portion with a substantial uniformity of pressure maintained throughout said passage through said portions oi the catalyst.

2. 'I'he process oi' producing ammonia by passing a. gaseous mixture oi' nitrogen and hydrogen over a catalyst mass at high temperatures under pressures below 400 atmospheres which comprises first passing preheated nitrogen hydrogen mixture through a separated portion of the catalyst mass, then introducing cooler nitrogen hydrogen mixture to the outiiowing mixture and thereafter passing the combined gas flow mixture through another separated portion .of the catalyst of greater content than said rst-mentioned portion with a substantial uniformity of pressure maintained throughout said passage through said portions of the catalyst;

3. In the process of producing ammonia by passing a gaseous mixture of nitrogen and hydrogen over a catalyst mass at high temperature under pressure below 400 atmospheres, the steps, which comprise passing the gas mixture into direct reaction contact with a portion of the catalyst mass, and then introducing additional, comparatively cooler nitrogen hydrogen mixture to the reacted gas flow from said portion in controllable amounts and passing the combined flow through other spaced-apart portions of the catalyst for further reaction while maintaining a continuous circulation therethrough.

4. In the process oi' producing ammonia by passing a gaseous mixture of nitrogen and hydrogen over a catalyst mass at high temperature under pressure below 400 atmospheres, the steps which comprise passing the gas mixture into direct reaction contact with a portion of the catalyst mass, and then introducing additional comparatively cooler nitrogen hydrogen mixture at a substantial uniformity of pressure to the reacted gas ilow from said portion in controllable amounts and passing the combined iiow through other spaced-apart portions of the catalyst for further reaction while maintaining a continuous circulation therethrough.

5. In the process of producing ammoniaby passing a gaseous mixture of nitrogen andy hydrogen over a catalyst mass at high temperature under pressure below 400 atmospheres, the steps which comprise passing the gas mixture into direct reaction contact with a portion of the catalyst mass, and then introducing variable quantities of comparatively cooler nitrogen hydrogen mixture to the reacted gas flow from said portion in controllable amounts and passing the combined iiow through other spaced-apart porvtions oi' the catalyst for further reaction while maintaining a continuous circulation therethrough. i

6. In the process of producingammonia by passing a gaseous mixture of nitrogen and hydrogen over a catalyst mass at high temperature under pressure below 400 atmospheres, the steps which comprise passing the gas mixture into direct reaction contact with a portion of the catalyst mass, and then introducing variable quantities of'comparatively cooler nitrogen hydrogen mixture at a substantial uniformity ot pressure to the reacted gas iiow from said portion in controllable amounts and passing the combined ilow through other spaced-apart portions of the catalyst for further reaction while maintaining a continuous circulation therethrough.

7. In the process of producing ammonia by passing a gaseous mixture of nitrogen and hydrogen over a catalyst mass at high temperature under pressure below 400 atmospheres, the steps which comprise passing the gas mixture into direct reaction contact with a portion of the catalyst mass, and then introducing additional comparatively cooler nitrogen hydrogen mixture to the reacted gas ilow from said portion in controllable amounts and passing the ycombined ilow through other spaced-apart portions of the catalyst for further reaction While .maintaining a continuouscirculation therethrough and a substantial uniformity of pressure during the passage of said gas mixture successively through said spaced-apart portions oi the catalyst mass.

8. In the process of producing ammonia by passing a gaseous mixture of nitrogen and hydrogen over a catalyst mass at high temperature under pressure below 400 atmospheres, the steps which comprise passing the gas mixture into direct reaction contact with a portion of the catalyst mass, and then introducing variable quantities of comparatively cooler nitrogen hydrogen mixture to the reacted gas flow from said portion in controllable amounts and passing the combined flow through other spaced-apart portions of the catalyst for further reaction while maintaining a continuous circulation therethrough and a substantial uniformity of pressure during the passage of said gas mixtures successively through said spaced-apart portions of the catalyst mass.v v

9. In the proces's of producing ammonia by passing a gaseous mixture oi nitrogen and hydrogen over a catalyst mass at high temperature under pressure below 400 atmospheres, the steps which comprise passing the gas mixture into direct reaction contact with a portion of the catalyst mass, and then introducing additional comparatively cooler nitrogen hydrogen mixture to the reacted gas ow from said portion in controllable amounts and passing the combined flow through other spaced-apart portions ot the catalyst for further reaction, said controllable amounts being brought indirectly into contact with said spaced-apart portions oi the catalyst, while maintaining a continuous circulation therethrough.

10. In the process of producing ammonia by passing a gaseous mixture oi nitrogen and hydrogen over a catalyst mass at high temperature under pressure below 400 atmospheres, the steps which comprise passing the gas mixture into direct reaction contact with a portion oi' the catalyst mass, and then introducing variable quantities of comparatively cooler nitrogen hydrogen mixture 'to the reacted gas flow from said portion in controllable amounts and passing the combined iiow through othery spaced-apart portions of the catalyst for further reaction, said controllable amounts being broughty indirectly into contactl with said spaced-apart portions o! the catalyst,

while mslnteinlnc s oontimmus circulation therethroush.

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bue synthesis under conditions ot high temnowinzfromthesddoatelystmw.mdthere -etternowinzthismixturethrouxhseeoondand separated cstelystmusgrester inextent than the former. while mxlntemlng s continuous cil'-, culatlontherethrough.

RALPH B. RICHARDSON. 

